Zwitterionic Covalent Organic Frameworks as Catalysts for Hierarchical Reduction of CO2 with Amine and Hydrosilane

2018 ◽  
Vol 10 (48) ◽  
pp. 41350-41358 ◽  
Author(s):  
Zhen-Jie Mu ◽  
Xuesong Ding ◽  
Zhi-Yan Chen ◽  
Bao-Hang Han
Keyword(s):  
Covalent Organic Frameworks ◽  
Reduction Of Co2 ◽  
Hierarchical Reduction

Transition-Metal-Free Catalysis for the Reductive ­Functionalization of CO2 with Amines

Synlett ◽  
2018 ◽  
Vol 29 (05) ◽  
pp. 548-555 ◽  
Author(s):  
Liang-Nian He ◽  
Xiao-Fang Liu ◽  
Xiao-Ya Li ◽  
Chang Qiao
Keyword(s):  
Transition Metal ◽  
Energy Content ◽  
Bond Formation ◽  
Energy Storage Materials ◽  
One Pot ◽  
Metal Free ◽  
Recent Developments ◽  
Electron Reduction ◽  
Reduction Of Co2 ◽  
Hierarchical Reduction

Reductive functionalization of CO2 with amines and a reductant, which combines both reduction of CO2 and C–N bond formation in one pot to produce versatile chemicals and energy-storage materials such as formamides, aminals, and methylamines that are usually derived from petroleum feedstock, would be appealing and promising. Herein, we give a brief review on recent developments in the titled CO2 chemistry by employing transition-metal-free catalysis, which can be catalogued as below according to the diversified energy content of the products, that is formamides, aminals, and methylamines being consistent with 2-, 4-, and 6-electron reduction of CO2, respectively. Notably, hierarchical reduction of CO2 with amines to afford at least two products, for example, formamides and methylamines, could be realized with the same catalyst through tuning the hydrosilane type, reaction temperature, or CO2 pressure. Finally, the opportunities and challenges of the reductive functionalization of CO2 with amines are also highlighted.1 Introduction2 2-Electron Reduction of CO2 to Formamide3 6-Electron Reduction of CO2 to Methylamine4 4-Electron Reduction of CO2 to Aminal5 Hierarchical Reduction of CO2 with Amines6 Conclusion

Catalyst-free hierarchical reduction of CO2 with BH3N(C2H5)3 for selective N-methylation and N-formylation of amines

2021 ◽  
Vol 50 ◽  
pp. 101590
Author(s):  
Qizhuang Zou ◽  
Yun Yi ◽  
Tianxiang Zhao ◽  
Fei Liu ◽  
Chao Kang ◽  
...  
Keyword(s):  
Catalyst Free ◽  
Reduction Of Co2 ◽  
Hierarchical Reduction

scholarly journals Covalent Organic Frameworks for the Capture, Fixation, or Reduction of CO2

2019 ◽  
Vol 7 ◽  
Author(s):  
John Ozdemir ◽  
Imann Mosleh ◽  
Mojtaba Abolhassani ◽  
Lauren F. Greenlee ◽  
Robert R. Beitle ◽  
...  
Keyword(s):  
Covalent Organic Frameworks ◽  
Reduction Of Co2

scholarly journals Covalent Organic Frameworks Linked by Amine Bonding for Concerted Electrochemical Reduction of CO2

Chem ◽  
2018 ◽  
Vol 4 (7) ◽  
pp. 1696-1709 ◽  
Author(s):  
Haoyu Liu ◽  
Jun Chu ◽  
Zhenglei Yin ◽  
Xin Cai ◽  
Lin Zhuang ◽  
...  
Keyword(s):  
Electrochemical Reduction ◽  
Covalent Organic Frameworks ◽  
Reduction Of Co2

Covalent organic frameworks: an ideal platform for designing ordered materials and advanced applications

2021 ◽  
Author(s):  
Ruoyang Liu ◽  
Ke Tian Tan ◽  
Yifan Gong ◽  
Yongzhi Chen ◽  
Zhuoer Li ◽  
...  
Keyword(s):  
Covalent Organic Frameworks ◽  
2D And 3D ◽  
Advanced Applications

Covalent organic frameworks offer a molecular platform for integrating organic units into periodically ordered yet extended 2D and 3D polymers to create topologically well-defined polygonal lattices and built-in discrete micropores and/or mesopores.

Intercalation of First Row Transition Metals inside Covalent-Organic Frameworks (COF): a Strategy to Fine Tune the Electronic Properties of Porous Crystalline Materials

2018 ◽  
Author(s):  
Srimanta Pakhira ◽  
Jose Mendoza-Cortes
Keyword(s):  
Transition Metal ◽  
Transition Metals ◽  
Electronic Properties ◽  
High Surface ◽  
Electronic Devices ◽  
High Surface Area ◽  
Main Role ◽  
Covalent Organic Frameworks ◽  
Porous Network ◽  
Crystalline Materials

<div>Covalent organic frameworks (COFs) have emerged as an important class of nano-porous crystalline materials with many potential applications. They are intriguing platforms for the design of porous skeletons with special functionality at the molecular level. However, despite their extraordinary properties, it is difficult to control their electronic properties, thus hindering the potential implementation in electronic devices. A new form of nanoporous material, COFs intercalated with first row transition metal is proposed to address this fundamental drawback - the lack of electronic tunability. Using first-principles calculations, we have designed 31 new COF materials <i>in-silico</i> by intercalating all of the first row transition metals (TMs) with boroxine-linked and triazine-linked COFs: COF-TM-x (where TM=Sc-Zn and x=3-5). This is a significant addition considering that only 187 experimentally COFs structures has been reported and characterized so far. We have investigated their structure and electronic properties. Specifically, we predict that COF's band gap and density of states (DOSs) can be controlled by intercalating first row transition metal atoms (TM: Sc - Zn) and fine tuned by the concentration of TMs. We also found that the $d$-subshell electron density of the TMs plays the main role in determining the electronic properties of the COFs. Thus intercalated-COFs provide a new strategy to control the electronic properties of materials within a porous network. This work opens up new avenues for the design of TM-intercalated materials with promising future applications in nanoporous electronic devices, where a high surface area coupled with fine-tuned electronic properties are desired.</div>

Seeded Growth of Single-Crystal Two-Dimensional Covalent Organic Frameworks

2017 ◽  
Author(s):  
Austin M. Evans ◽  
Lucas R. Parent ◽  
Nathan C. Flanders ◽  
Ryan P. Bisbey ◽  
Edon Vitaku ◽  
...  
Keyword(s):  
Molecular Transport ◽  
Controlled Synthesis ◽  
Two Dimensional ◽  
Covalent Organic Frameworks ◽  
Seeded Growth ◽  
Covalent Bonds ◽  
Crystalline Materials ◽  
Step Procedure ◽  
Structures And Properties ◽  
2D Polymer

<div> <div> <div> <p>Polymerizing monomers into periodic two-dimensional (2D) networks provides structurally precise, atomically thin macromolecular sheets linked by robust, covalent bonds. These materials exhibit desirable mechanical, optoelectrotronic, and molecular transport properties derived from their designed structure and permanent porosity. 2D covalent organic frameworks (COFs) offer broad monomer scope, but are generally isolated as polycrystalline, insoluble powders with limited processability. Here we overcome this limitation by controlling 2D COF formation using a two- step procedure. In the first step, 2D COF nanoparticle seeds are prepared with approximate diameters of 30 nm. Next, monomers are slowly added to suppress new nucleation while promoting epitaxial growth on the existing seeds to sizes of several microns. The resulting COF nanoparticles are of exceptional and unprecedented quality, isolated as single crystalline materials with micron-scale domain sizes. These findings advance the controlled synthesis of 2D layered COFs and will enable a broad exploration of synthetic 2D polymer structures and properties. </p> </div> </div> </div>

Seeded Growth of Single-Crystal Two-Dimensional Covalent Organic Frameworks

2017 ◽  
Author(s):  
Austin M. Evans ◽  
Lucas R. Parent ◽  
Nathan C. Flanders ◽  
Ryan P. Bisbey ◽  
Edon Vitaku ◽  
...  
Keyword(s):  
Molecular Transport ◽  
Controlled Synthesis ◽  
Two Dimensional ◽  
Covalent Organic Frameworks ◽  
Seeded Growth ◽  
Covalent Bonds ◽  
Crystalline Materials ◽  
Step Procedure ◽  
Structures And Properties ◽  
2D Polymer

<div> <div> <div> <p>Polymerizing monomers into periodic two-dimensional (2D) networks provides structurally precise, atomically thin macromolecular sheets linked by robust, covalent bonds. These materials exhibit desirable mechanical, optoelectrotronic, and molecular transport properties derived from their designed structure and permanent porosity. 2D covalent organic frameworks (COFs) offer broad monomer scope, but are generally isolated as polycrystalline, insoluble powders with limited processability. Here we overcome this limitation by controlling 2D COF formation using a two- step procedure. In the first step, 2D COF nanoparticle seeds are prepared with approximate diameters of 30 nm. Next, monomers are slowly added to suppress new nucleation while promoting epitaxial growth on the existing seeds to sizes of several microns. The resulting COF nanoparticles are of exceptional and unprecedented quality, isolated as single crystalline materials with micron-scale domain sizes. These findings advance the controlled synthesis of 2D layered COFs and will enable a broad exploration of synthetic 2D polymer structures and properties. </p> </div> </div> </div>

Graphene Supported Tungsten Carbide as Catalyst for Electrochemical Reduction of CO2

2019 ◽  
Author(s):  
Sahithi Ananthaneni ◽  
Rees Rankin
Keyword(s):  
Tungsten Carbide ◽  
Electrochemical Reduction ◽  
Low Cost ◽  
Co2 Reduction ◽  
Platinum Group Metal ◽  
Reduction Reaction ◽  
Metal Carbides ◽  
Depth Study ◽  
Reduction Of Co2 ◽  
Co2 Reduction Reaction

<div>Electrochemical reduction of CO2 to useful chemical and fuels in an energy efficient way is currently an expensive and inefficient process. Recently, low-cost transition metal-carbides (TMCs) are proven to exhibit similar electronic structure similarities to Platinum-Group-Metal (PGM) catalysts and hence can be good substitutes for some important reduction reactions. In this work, we test graphenesupported WC (Tungsten Carbide) nanocluster as an electrocatalyst for the CO2 reduction reaction. Specifically, we perform DFT studies to understand various possible reaction mechanisms and determine the lowest thermodynamic energy landscape of CO2 reduction to various products such as CO, HCOOH, CH3OH, and CH4. This in-depth study of reaction energetics could lead to improvements and develop more efficient electrocatalysts for CO2 reduction.<br></div>

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